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This thesis describes the results of angle resolved photoemission spectroscopy experiments on delafossite oxide metals, and theoretical work explaining these observations. The study was motivated by the extraordinarily high conductivity of the non-magnetic delafossites PdCoO2 and PtCoO2, the measurement of whose electronic structure is reported and discussed. Two unexpected effects were observed in the course of the investigation; each is described and analysed in detail. Firstly, a previously unrecognised type of spectroscopic signal, allowing the non-magnetic probe of photoemission to become sensitive to spin-spin correlations, was observed in the antiferromagnetic PdCrO2. Its origin was identified as the Kondo-like coupling of itinerant and Mott insulating electrons. Furthermore, surface states exhibiting an unusually large Rashba-like spin-splitting were observed on the transition metal terminated surfaces of delafossites. The large inversion symmetry breaking energy scale, a consequence of the unusual structure of the surface layer, is identified as the origin of the effect.
Solid state physics. --- Spectroscopy. --- Microscopy. --- Materials—Surfaces. --- Thin films. --- Solid State Physics. --- Spectroscopy and Microscopy. --- Surfaces and Interfaces, Thin Films. --- Spectroscopy/Spectrometry. --- Films, Thin --- Solid film --- Solid state electronics --- Solids --- Surfaces (Technology) --- Coatings --- Thick films --- Analysis, Microscopic --- Light microscopy --- Micrographic analysis --- Microscope and microscopy --- Microscopic analysis --- Optical microscopy --- Optics --- Analysis, Spectrum --- Spectra --- Spectrochemical analysis --- Spectrochemistry --- Spectroscopy --- Chemistry, Analytic --- Interferometry --- Radiation --- Wave-motion, Theory of --- Absorption spectra --- Light --- Spectroscope --- Physics --- Qualitative --- Photoelectron spectroscopy. --- Spectroscopy, Photoelectron --- Electron spectroscopy --- Molecular orbitals --- Molecular spectra --- Molecular spectroscopy --- Photoelectricity --- Spectrum analysis --- Spectrometry --- Analytical chemistry
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Electrochemical surface science (EC-SS) is the natural advancement of traditional surface science (where gas–vacuum/solid interfaces are studied) to liquid (solution)/electrified solid interfaces. Such a merging between two different disciplines—i.e., surface science (SS) and electrochemistry—officially advanced ca. three decades ago. The main characteristic of EC-SS versus electrochemistry is the reductionist approach undertaken, inherited from SS and aiming to understand the microscopic processes occurring at electrodes on the atomic level. A few of the exemplary keystone tools of EC-SS include EC-scanning probe microscopies, operando and in situ spectroscopies and electron microscopies, and differential EC mass spectrometry (DEMS). EC-SS indirectly (and often unconsciously) receives a great boost from the requirement for rational design of energy conversion and storage devices for the next generation of energetic landscapes. As a matter of fact, the number of material science groups deeply involved in such a challenging field has tremendously expanded and, within such a panorama, EC and SS investigations are intimately combined in a huge number of papers. The aim of this Special Issue is to offer an open access forum where researchers in the field of electrochemistry, surface science, and materials science could outline the great advances that can be reached by exploiting EC-SS approaches. Papers addressing both the basic science and more applied issues in the field of EC-SS and energy conversion and storage materials have been published in this Special Issue.
Pd thin films --- n/a --- Auger-Electron Spectroscopy --- benchmarking --- potential-dependent structures --- CO electro-oxidation --- surface reconstruction --- photo-electrochemistry --- nitrogen doping --- potential stepping --- DFT --- nanoparticles --- carbon nanofiber --- Pd --- gas diffusion electrode --- flexible ITO --- UPS --- palladium --- Lead OPD --- formic acid oxidation --- cobalt oxide --- adsorbed OH --- electrochemistry --- Pt --- mesopore --- DMFC --- pH and concentration effects --- solvothermal method --- direct methanol fuel cells --- EF-PEEM --- PVDF --- self-assembly --- PEMFC --- hard X rays --- photochemistry --- EQCM --- potential cycling --- surface alloy --- near ambient pressure XPS --- cobalt-based electrocatalyst --- silver single crystals --- Cu(111) --- electrodeposited alloys --- Pt single-crystal electrodes --- SOFC --- TiO2 --- oxygen evolution reaction --- silicon nanoparticles --- pump & --- graphitization --- in situ EC-STM --- oxygen reduction --- gold --- diazonium salts --- Au --- micropore --- solid/liquid interface --- XPS --- XAFS --- surface chemistry --- electrosynthesis --- porous fiber --- surface science --- click chemistry --- adhesion --- in situ --- methanol oxidation reaction --- hydroxyl radical --- mass transport --- free electron laser --- cyclic voltammetry --- redox properties --- electro-oxidation --- X-ray absorption spectroscopy --- hydrogen adsorption --- electrodeposition --- electrocatalysis --- Ordered mesoporous carbon --- Corrosion Protection --- electrochemical interface --- cyclic voltammetry (CV) --- FEXRAV --- photoelectron simulations --- Pt–Ru catalysts --- d-band theory --- bimetallic alloy --- photoconversion --- ordered mesoporous carbons --- carbon nanofibers (CNFs) --- platinum --- water splitting --- Surface Modification --- EPR spectroscopy --- scanning photoelectron microscopy --- model catalyst --- energy dispersive --- porphyrins --- combined non-covalent control --- AES --- spin-coating --- SAMs --- water oxidation --- in-situ X-ray diffraction --- Au nanocrystals --- model systems --- platinum single crystals --- cathode --- redox monolayers --- surface nanostructures --- bifunctional oxygen electrode --- polymer --- photoelectrochemistry --- metal-electrolyte interface --- electrocatalysts --- APTES --- porogen --- electrophoretic deposition --- thin-films --- ammonia activation --- graphene --- ORR --- polypyrrole --- iridium --- surface area --- reduced graphene oxide --- Magnetite --- Platinum --- electrospinning --- catalysts --- Blackening of Steel --- switchable surfaces --- in situ ambient pressure XPS --- fuel cells --- methanol oxidation --- quick-XAS --- nickel --- CO oxidation --- solid oxide fuel cells --- operando --- probe --- CdS --- alkanthiols --- ECALE --- alkoxyamine surfaces --- underpotential deposition (upd) --- Pt-Ru catalysts
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